新型无机固体吸附剂在天然气脱水领域研究进展

doi:10.19964/j.issn.1006-4990.2021-0756

摘要/Abstract

摘要：

天然气在进入管网输送之前必须经过脱水处理，目前常用的天然气脱水方法主要有冷干法、液体吸收法和固体吸附法。用于天然气脱水的固体吸附剂主要包括分子筛、氧化铝、介孔二氧化硅和金属有机框架材料（MOFs）等。随着更多海上气田的勘探开发，分子筛和氧化铝等传统吸附剂已无法满足对大量天然气的净化需求，需要使用具有更高负载能力的吸附剂。介孔二氧化硅和MOFs具有高化学稳定性、低密度、高孔隙度的优点，且使用寿命长，避免了频繁更换，作为天然气脱水吸附剂具有潜在优势。围绕高比表面积、孔体积、亲水性和再生能力等综述了介孔二氧化硅和金属有机框架材料（MOFs）在天然气脱水方面的研究进展。介孔二氧化硅具有良好的亲水性和机械稳定性，可在高压力范围内使用，提升处理装置的效率。然而介孔二氧化硅主要是通过溶胶-凝胶法合成，老化时间较长，且传统的蒸发干燥法无法保持完全凝胶的结构。未来有望通过超临界流体干燥法获得具有更好物化性质和孔结构的介孔二氧化硅，进一步提高介孔二氧化硅的吸附能力。MOFs作为无机物和有机物结合形成的多孔材料，具有高度规则的孔结构和可调的性质，且金属离子与配体官能团的自由电子对之间的化学或物理相互作用，使其具有较高的天然气吸附脱水效率和优异的再生循环性能。最后指出，需要进一步研究复杂工况下的MOFs吸附脱水能力、长周期运行稳定性以及高压工况、造粒及不同分离过程（变压吸附和变温吸附）对MOFs的影响，并开发MOFs低成本规模化制备技术实现工业化应用。

关键词: 无机固体吸附剂, 介孔二氧化硅, 金属有机框架材料, 天然气脱水

Abstract:

Natural gas must be dehydrated before entering the pipeline network.At present，the commonly used natural gas dehydration methods mainly include cold dry method，liquid absorption method and solid adsorption method.Solid adsorbents for natural gas dehydration mainly include zeolite，alumina，mesoporous silica and metal organic framework materials （MOFs）.With the exploration and development of more offshore gas fields，traditional adsorbents such as zeolite and alumina can not meet the purification needs of a large amount of natural gas，so adsorbents with higher loading capacity need to be used.Mesoporous silica and MOFs have the advantages of high chemical stability，low density，high porosity and long service life，and avoid frequent replacement，which have potential advantages as natural gas dehydration adsorbents.The research progress of mesoporous silica and MOFs in natural gas dehydration was reviewed by focusing on high specific surface area，pore volume，hydrophilicity and regeneration ability in this paper.Mesoporous silica had good hydrophilicity and mechanical stability，which could be used in high pressure range to improve the efficiency of the treatment device.However，mesoporous silica was mainly synthesized by sol-gel method，and the aging time was longer.The traditional evaporation drying method could not maintain the complete gel structure.In the future，mesoporous silica with better physicochemical properties and pore structure was expected to be obtained by supercritical fluid drying，so as to further improve the adsorption capacity of mesoporous silica.As porous materials formed by the combination of inorganic and organic substances，MOFs had highly regular pore structure and adjustable properties，and the chemical or physical interaction between metal ions and free electron pairs of ligand functional groups made them have high natural gas adsorption and dehydration efficiency and excellent regeneration cycle performance.Finally，it was pointed out that it was necessary to further study the adsorption and dehydration capacity of MOFs under complex working conditions，long-term operation stability，and the effect of high-pressure working conditions，granulation and different separation processes（PSA and TSA） on MOFs，and develop low-cost and large-scale preparation technology of MOFs to realize industrial application.

Key words: inorganic solid adsorbent, mesoporous silica, metal organic framework materials, natural gas dehydration

中图分类号:

TQ127.2

石涵,袁标,沈鹏. 新型无机固体吸附剂在天然气脱水领域研究进展[J]. 无机盐工业, 2022, 54(5): 11-18.

SHI Han,YUAN Biao,SHEN Peng. Research progress on new inorganic solid adsorbents in field of natural gas dehydration[J]. Inorganic Chemicals Industry, 2022, 54(5): 11-18.

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材料	比表面积/（m²·g^-1）	孔体积/（cm³·g^-1）	孔径/ nm	密度/ （kg·m^-3）	再生温度/℃
分子筛	300~800	0.27~0.45	2~50	690~1 000	150~290
氧化铝	210	2.6	2.6	801~881	220~320
介孔二氧化硅	600~1 300	0.40~0.45	2~8	720~800	120~230
MOFs	1 000~4 000	0.53~1.36	0.3~3.6	700~900	100~170

样品	操作条件			吸附能力/ （g·g^-1）
样品	室温湿度/%	温度/℃	p/p₀	吸附能力/ （g·g^-1）
F127-SiO₂^［30］	84	25	0.9	0.45
Brij56-SiO₂^［30］	84	25	0.9	0.25
SBA-15^［31］	—	20	0.9	0.084
SBA-15^［32］	90	35	0.9	0.54
SiO₂/CaCl₂^［33］	60	40	0.9	0.47
AlFFIVE-1-Ni （KAUST-8）^［26］	95	35	0.9	0.27
MOF-303^［34］	94	15	0.3	0.48
HKUST-1^［35］	—	25	0.9	0.55
MIL-100（Fe）^［35］	—	25	0.9	0.81
MIL-101^［35］	—	25	0.9	1.28
DUT-4^［35］	—	25	0.9	0.28
ZIF-8^［35］	—	25	0.9	0.02
MIL-101^［36］	—	25	0.9	1.2
MIL-101（Cr）^［37］	60	30	0.57	1.5
MIL-101（Cr）-NH₂^［38］	—	20	0.4	1.06
MOF-801^［27］	100	25	0.9	0.05
MOF-808^［27］	100	25	0.9	0.08
MOF-841^［27］	100	25	0.9	0.07
MIL-101（Cr）/CaCl₂^［39］	—	25	0.9	2.2

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